UV-Vis Nadir Retrievals

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1 SCIAMACHY book UV-Vis Nadir Retrievals Michel Van Roozendael, BIRA-IASB ATC14, October, Jülich, Germany

2 Introduction Content Fundamentals of the DOAS method UV-Vis retrievals: from simplified to more advanced approaches Limits of DOAS Beyond/advanced DOAS 2

3 Introduction/ history 1879 Marie Alfred Cornu postulates the existence of a protecting UV-absorbing species in the atmosphere 1880 Sir Walther Noel Hartley identifies the presence of ozone from spectroscopic observations 1908 Léon Teisserenc de Bort locates the ozone layer (10-50 km) based on balloon-borne temperature measurements 1925 Gordon Dobson develops a new very stable total ozone instrument (still used today) and defines the reference unit for the ozone layer thickness 1973 Alan Brewer designs an improved total ozone spectrometer, similar to Dobson but more accurate and automated 1975 J.F. Noxon introduces the first NO 2 measurements using sky radiances 1976 Ulrich Platt and Dieter Perner introduce the DOAS method, first applied to tropospheric observations using artificial light sources 1985 Discovery of the Ozone hole, DOAS instruments are increasingly developed to monitor the atmospheric composition from various platforms 3

4 Simplified representation of the UV-Vis radiative transport in nadir viewing geometry 0 Z Gas layer Surface In first approximation the problem is equivalent to treating the attenuation of a light ray through a gas cell 4

5 The Beer-Lambert law Light source I o (λ) Absorber of concentration c and cross-section σ(λ) Spectrometer I(λ) Cell of length L I( λ) = I 0 ( λ) e c L σ ( λ ) I0( λ) c L σ ( λ) = ln I( λ) τ = optical thickness : can be used to derive c or σ(λ) 5

6 Absorption cross-sections Molecular absorption characterised by specific spectral features molecule fingerprint UV-Vis cross-sections independent of pressure and weakly dependent on temperature (can be linearised) Molecules absorbing in UV- Vis are generally shortlived 6

7 Differential Optical Absorption Spectroscopy (DOAS) More realistic expression for the atmospheric attenuation: Trace gases Rayleigh scattering ~ λ -4 Mie Scattering ~ λ -(1 3) I λ = I 0 (λ) e σ i λ c i L + ε RRR λ +ε MMM λ L the DOAS approach (frequency separation): I λ = I 0 (λ) e σ i λ c i L + σ bb λ + ε RRR λ +ε MMM λ L High frequency broadband band extinction Remove by high-pass filtering

8 Exemple of DOAS frequency separation Intensity (a.u.) O 3 transmission Polynomial 3 rd degree 8 Differential spectrum

9 DOAS evaluation method I ( λ) = I ( λ) 0 e L j σ j ( λ ) c L σ ( λ ) j i 0 j c j + ε + ε R M ( ) ( ) I 0 λ D meas. ( λ ) = ln L = σj ( λ ) c j + L σ0 j ( λ ) c j +ε R +ε M + ln A ( λ I λ j j Differential Part Continuous Part D λ = a σ λ + b λ = Modeled spectrum ( ) ( ) k Fit i i k i k Slant columns (SCD i ) Differential Part Polynomial models Continuous Part 9

10 Exemple of DOAS retrieval (NO 2 ) QDOAS software 10

11 The solar spectrum as a light source Difficulties: Multitude of solar lines (Fraunhofer lines) Solar lines are Doppler shifted must be corrected Spectrum varies over the disk Some variations in intensity Advantages: Maximum intensity in visible Fraunhofer lines can be used as a reference for wavelength and resolution 11

12 Wavelength calibration/ shift-stretch Wavelength calibration of spectrometers usually determined in the lab using monochromatic emission lines of know position For DOAS, it is essential that measured spectra and reference laboratory cross-sections are always perfectly aligned with each other Misalignments may occur due to, e.g. Doppler shift related to earth rotation, thermal instabilities, instrument degradation, inaccuracies in laboratory data, etc In advanced DOAS retrievals, wavelength shift (and stretch) are dynamically adjusted using solar lines as reference (see practical for details) 12

13 Instrument Response Function (IRF) The Instrument Response Function IRF (often also called slit function) is the response of the instrument to a monochromatic input: The IRF is usually measured pre-flight in the lab Its knowledge is critical for DOAS retrievals The IRF can be altered due to thermal instabilities or instrument degradation It may also depend on how well the entrance aperture is illuminated ( problems with partially cloudy skies) The IRF can be monitored using solar lines as reference (see practical for more details) Solar spectra at different resolution high-resolution convolved 13

14 Because of the finite resolution of the DOAS spectrometers, the Fraunhofer lines and the absorption by molecules can interfere (solar I 0 effect): Real Intensity: Measured intensity: Measured reflectance: Solar I 0 effect I( λ) = I0( λ)exp{ σ ( λ) L} [ I ( λ)exp{ σ ( λ) }] [ I ( λ)exp{ σ ( λ) L} ] I *( λ) = F * 0 L *( λ) F * 0 = 0 *( λ) F * I0( λ)} I I Only if either I 0 or exp{-σl} varies slowly, they can be moved out of the integral so the standard DOAS approach holds: I *( λ) log F * σ ( λ) L I *( λ) for strong differential absorption and close to strong solar lines a correction is needed which can be computed by simulating the effect 0 14

15 Temperature dependence of absorption cross-sections σ λ, T = σ λ, T 0 + T T 0 σ T 330 nm log I I 0 = σ λ, T S log I I 0 = σ λ, T 0 S + T T 0 S B Effective temperature: T = T 0 + B/S 15

16 QDOAS software (practical) Generic DOAS retrieval software developed at BIRA, and S&T (GUI) Comprehensive functionalities for all type of DOAS applications Ingest most UV-Vis sensors (GOME, SCIA, OMI, GOME-2) 16

17 Geometrical Air Mass Factor (AMF G ) SZA θ LOS ϕ A AMF G = 1 cos( θ ) + 1 cos( ϕ) clearly wrong for low sun! Accounting for sphericity, SZA and LOS depend on altitude with larger values in the lowest layers 17

18 More realistic view of the UV-Vis radiative transfer in the earth atmosphere Absorption Scattering from a cloud Transmission through a cloud Atmosphere Scattering Aerosol / Molecules Scattering / reflection oh a cloud Cloud Scattering within a cloud Transmission through a cloud Absorption on the ground Scattering / Reflection on the ground 18

19 Radiative transfer equation 19 Express the variation of the diffuse radiation in height z at one wavelength: ) ( ) ( ),,,, ( ) ( ),,,, ( ) ( ),, ( ),,,, ( ) ( ),, ( )) ( ) ( ( ),, ( ))/ ( ( / )/ ( B T z Ae z P d d e F z e F z P z z I z P d d z z I z z z I dz d z sol z sol ε ϕ µ ϕ µ µ ϕ π ς ϕ µ ϕ µ π ς ϕ µ ϕ µ ϕ µ µ ϕ π ς ϕ µ ς ε ϕ µ µ µ τ τ π µ τ µ τ π = Θ zenith angle µ cos(θ) ϕ azimuth angle ε emission coefficient (= absorption coefficient) ζ scattering coefficient Fsol flux from the sun P weighted phase function for scattering A surface albedo B Planck radiation τ optical depth loss by extinction gain by multiple scattering gain by single scattering of solar radiation gain by reflection of light from the surface gain by emission

20 Optically thin approximation and concept of effective photon path length In a large part of the UV and visible range, the optical thickness of the atmosphere is small and dominated by scattering (Rayleigh and Mie) and reflection at the surface and from clouds As a result, the radiative transfer is weakly dependent on the abundance of minor absorbers present in the atmosphere, and also weakly dependent on the wavelength (at least for small intervals used in DOAS) Therefore one can define one effective photon path length which is representative of the mean light path at one wavelength (generally the central wavelength of the DOAS interval) This allows to maintain a convenient separation between the DOAS retrieval part and the treatment of the radiative transfer, which is done in a separate step using complex radiative transfer models. 20

21 Air Mass Factor (AMF) definition The AMF is defined as the ratio of the measured slant column to the vertical column in the atmosphere: The AMF expresses the sensitivity of the measurement, and depends on a variety of parameters such as: wavelength geometry vertical distribution of the species clouds aerosol loading surface albedo AMF = SC( λ, Θ,...) VC Because of the optically thin approximation, the AMF depends weakly on the vertical column the idea is that if all other dependences are known, the measured signal is proportional to the VC. 21

22 AMF calculation AMF are generally calculated by performing two radiative transfer calculations, one with and one without the absorber of interest: I + = radiance with absorber I - = radiance without absorber AAA λ, θ = log I λ, θ I + λ, θ σ(λ) VV works well for optically thin situations 22

23 AMF dependences AMFs strongly depend on the altitude At high 340 nm altitude (stratosphere), the SZA dominates the geometry At low altitude (troposphere) scattering and surface reflection effects dominate. Scattering effects are increasingly dominant at shorter wavelength (σ Ray ~ 1/λ 4 ). Over dark surfaces, the sensitivity to near surface absorbers is lowest in the UV. A In good approximation, an AMF can be calculated for each layer, and the total AMF is then given by: AMFi VCi The AMF i i are also often called AMF = VC Scattering Weights or Box AMFs i i 23

24 AMF i dependences (340 nm) SZA LOS RAA Albedo Altitude (low albedo) Altitude (high albedo) 24

25 Surface reflectivity In the UV-Vis region the surface reflectivity is generally low except over snow and ice covered areas 25

26 in percent! % 26

27 Clouds shield surface Treatment of clouds Clouds enhance sensitivity to absorbers located above or at cloud altitude (due to albedo effect) Stratospheric absorbers are weakly affected by clouds Clouds generally treated as lambertian reflectors in the independent pixel approximation: AAA = Φ = 1 Φ AAA ccccc + Φ AAA ccooo C f I ccccc 1 C f I cllll + C f I ccccc where Φ is the cloud radiance fraction 27

28 The Averaging Kernel (AK) concept The AK expresses the sensitivity of the retrieval in the vertical axis, or the way the retrieval smoothes the actual profile information For a DOAS retrieval: AA (z) = AAA (z) AAA The AK allows to account for the measurement sensitivity when performing a comparison with a reference profile (x ref ): V = AA x rrr Eskes and Boersma, ACP,

29 Ring effect In addition to elastic Rayleigh and Mie scattering, inelastic rotational Raman scattering on air molecules is also important in the atmosphere. Raman scattering moves energy from the incoming wavelength to neighbouring wavelengths and thus changes the spectral distribution in the scattered light. As a result, the solar lines are less deep in scattered light than in direct solar light. This was first observed Ring & Grainger in The degree of filling-in depends on the geometry of sun and observation, albedo, clouds.. It amounts to a few percent of the total scattered light. This smoothing effect must be corrected in the retrieval 29

30 Correction of Ring and molecular Ring effect Use of an effective Ring crosssection calculated using radiative transfer calculations including rotational Raman scattering In addition to the Ring effect introduced by the Fraunhofer lines, inelastic scattering also fills in the depth of trace gas absorptions (molecular Ring effect). For a stratospheric absorber, this can be corrected using: S cccc = S 1 1 ρ 0 (1 sec (θ) AAA ) 30

31 Ring effect in O 3 retrieval: example for one GOME-2 orbit High albedo and low sun Fitted Ring coefficient High clouds 1 1 ρ 0 (1 sec (θ) AAA ) 31

32 Stratosphere-troposphere separation Nadir UV-Vis observation do not carry information on the altitude The slant column signal results from reflection or scattering taking place close to the surface slant columns contain absorption in both the troposphere and the stratosphere Not a problem for tropospheric gases (e.g. SO 2, HCHO) For other molecules (e.g. NO 2, O 3, BrO) the stratospheric content is significant and must be removed before tropospheric retrieval 32

33 Residual tropospheric NO 2 retrieval Total NO 2 Stratospheric NO 2 Reference sector Tropospheric NO 2 33

34 Residual tropospheric BrO Stratospheric column derived from a climatology build on CTM simulations Theys et al., ACP,

35 Residual tropospheric BrO Theys et al., ACP,

36 Tropospheric ozone limb-nadir matching Ebojie et al., AMT,

37 Limits of the DOAS approximation The main limitation is related to the variation of the AMF with wavelength: in the presence of strong absorbers (O 3, O 2, H 2 O), the photon light path is affected by the absorber itself, leading to inaccuracies resulting from the change of airmass factor with wavelength in the case of (non-linear) temperature or pressure dependent cross-sections an additional error is introduced 37

38 Beyond DOAS: (1) Total ozone direct-fitting Use a radiative transport model as forward model and directly fit measured reflectances Better accuracy, especially for low sun conditions 38

39 Beyond DOAS: (2) SO 2 plume height retrieval For large SO 2 and ozone absorptions in the UV, the wavelength dependence of the SO 2 AMF becomes a strong function of the altitude This can be used to retrieve an information on the altitude of strong SO 2 volcanic plumes AMF AAA z Yang et al., JGR,

40 Beyond DOAS: (3) surface NO 2 identification In case of large surface NO 2 absorptions, the AMF becomes of strong function of the wavelength even in small intervals This can be used to identify hot spots of NO 2 emitted at the surface. This technique is under development in Bremen Richter, DOAS workshop,

41 Thank you for your attention Questions? 41

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